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arXiv:2308.00995 · Physical Review Letters

Transform-Limited Photon Emission from a Lead-Vacancy Center in Diamond above 10 K

Peng Wang, Lev Kazak, Katharina Senkalla, Petr Siyushev, Ryotaro Abe, Takashi Taniguchi, Shinobu Onoda, Hiromitsu Kato, Toshiharu Makino, Mutsuko Hatano, Fedor Jelezko, Takayuki Iwasaki

Published Feb 15, 2024• 25 citations
arXivHTMLPDF

Abstract

Transform-limited photon emission from quantum emitters is essential for high-fidelity entanglement generation. In this Letter, we report the coherent optical property of a single negatively charged lead-vacancy (PbV) center in diamond. Photoluminescence excitation measurements reveal stable fluorescence with a linewidth of 39 MHz at 6 K, close to the transform limit estimated from the lifetime measurement. We observe 4 orders of magnitude different linewidths of the two zero-phonon lines, and find that the phonon-induced relaxation in the ground state contributes to this huge difference in the linewidth. Because of the suppressed phonon absorption in the PbV center, we observe nearly transform-limited photon emission up to 16 K, demonstrating its high temperature robustness compared to other color centers in diamond.

DOI
10.1103/physrevlett.132.073601

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Transform-limited photon emission from quantum emitters is essential for high-fidelity entanglement generation. In this Letter, we report the coherent optical property of a single negatively charged lead-vacancy (PbV) center in diamond. Photoluminescence excitation measurements reveal stable fluorescence with a linewidth of 39 MHz at 6 K, close to the transform limit estimated from the lifetime measurement. We observe 4 orders of magnitude different linewidths of the two zero-phonon lines, and find that the phonon-induced relaxation in the ground state contributes to this huge difference in the linewidth. Because of the suppressed phonon absorption in the PbV center, we observe nearly transform-limited photon emission up to 16 K, demonstrating its high temperature robustness compared to other color centers in diamond.
We report on quantum emission from Pb-related color centers in diamond following ion implantation and high-temperature vacuum annealing. First-principles calculations predict a negatively charged Pb-vacancy (PbV) center in a split-vacancy configuration, with a zero-phonon transition around 2.4 eV. Cryogenic photoluminescence measurements performed on emitters in nanofabricated pillars reveal several transitions, including a prominent doublet near 520 nm. The splitting of this doublet, 5.7 THz, exceeds that reported for other group-IV centers. These observations are consistent with the PbV center, which is expected to have a combination of narrow optical transitions and stable spin states, making it a promising system for quantum network nodes.
A negatively charged lead-vacancy (PbV-) center in diamond is a novel quantum system which can be operated at a high temperature above 4 K owing to its large ground state splitting. To unlock the quantum properties of the PbV- center, the enhancement of the fluorescence intensity is a key issue. Here, we demonstrate enhanced emission from PbV- centers by a factor of approximately 10 using solid immersion lenses (SILs) fabricated on rough diamond surface caused by high-temperature anneal over 2000°C. Resonant excitation reveals the narrow emission close to the transform-limited linewidth. Furthermore, we demonstrate two-photon interference using one single PbV- center in an SIL. This enhanced emission and indistinguishability will lead to further development of the PbV- center towards quantum network node applications.
We report the optical observation of lead-vacancy (PbV) centers in diamond fabricated by Pb ion implantation and subsequent high-temperature annealing (2100 °C) under high pressure (7.7 GPa). Their optical properties were characterized by photoluminescence at varying temperatures down to 5.7 K. We observed intense emission peaks at 550 and 554 nm, with a large splitting of approximately 3900 GHz. The two lines are thought to correspond to the zero phonon line (ZPL) of PbV centers with split ground and excited states. A cubic trend of the ZPL width was observed while varying the temperature. We performed polarization measurements of the two lines in a single PbV center, showing nearly orthogonal dipole polarizations. These optical measurements strongly indicate that the PbV center possesses D 3 d symmetry in the diamond lattice. The observed large ground state splitting significantly suppresses the phonon-mediated transition, which causes decoherence of the electron spin state of the group IV color centers in diamond, leading to the expectation of a long spin coherence time at a temperature ∼9 K.
A lead-vacancy (PbV) center in diamond exhibits coherent emission above the liquid helium temperature, making it highly attractive for quantum network applications. Here, we report the magneto-optical and spin properties of PbV centers in diamond. We record a spin lifetime of 12 ms at 7.5 K under large off-axis magnetic field. Furthermore, we observe formation of the coherent dark state by coherent population trapping and estimate a spin dephasing time of 177 ns at 6.5 K. This work demonstrates the outstanding thermal robustness of the PbV spin compared to other group-IV centers above 4 K.
The realization of quantum networks is based on the entanglement of stationary qubits via flying photons. Therefore, a fundamental requirement is a single photon source that can efficiently generate indistinguishable photons for the entanglement generation. The group-IV vacancy centers in diamond have emerged as promising candidates due to their spectral stability benefiting from inversion symmetry and long spin coherence time. In particular, the lead-vacancy (PbV) center exhibits fourier-limited linewidths even above 10 K and is predicted to have millisecond-scale spin coherence time near 9 K, making it suitable for scalable quantum networks. Here, we report the indistinguishability of photons emitted from a single PbV center in diamond through a two-photon interference experiment, known as the Hong-Ou-Mandel (HOM) effect. Fluorescence from the PbV center was split into two paths and recombined at a HOM interferometer. Photon correlations were measured for parallel and orthogonal polarized schemes. In parallel polarization, a clear interference dip below 0.5 at zero time delay was observed, whereas for orthogonal polarization, the correlation function exceeded 0.5. These results confirm the generation of indistinguishable photons from a single PbV center, validating their potential as the solid-state quantum emitter. This work paves the way for the PbV-based application for quantum information processing.
The negatively charged nickel vacancy center (NiV^{-}) in diamond is a promising spin qubit candidate with predicted inversion symmetry, large ground state spin-orbit splitting to limit phonon-induced decoherence, and emission in the near infrared. Here, we experimentally confirm the proposed geometric and electronic structure of the NiV defect via magneto-optical spectroscopy. We characterize the optical properties and find a Debye-Waller factor of 0.62. Additionally, we engineer charge state stabilized defects using electrical bias in planar all-diamond p-i-p junctions. We measure a vanishing static dipole moment and no spectral diffusion, characteristic of inversion symmetry. Under bias, we observe stable transitions with lifetime-limited linewidths as narrow as 16 MHz and convenient frequency tuning of the emission via a second-order Stark shift. Overall, this Letter provides a pathway toward coherent control of the NiV^{-} and its use as a spin qubit and contributes to a more general understanding of charge dynamics experienced by defects in diamond.